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Item Room-temperature ultraviolet-ozone annealing of ZnO and ZnMgO nanorods to attain enhanced optical properties(Springer, 2020) Alam, M.J.; Murkute, P.; Sushama, S.; Ghadi, H.; Mondal, S.; Paul, S.; Das, D.; Pandey, S.K.; Chakrabarti, S.ZnO and ZnMgO nanorods have proven to be promising materials for sensing, UV and deep UV based optoelectronic applications. A major drawback of ZnO and ZnMgO based thin films and nanorods is the presence of native point defects which deteriorates their optical efficiency and becomes an impediment to their efficient device applications. The furnace and rapid thermal annealing processes have overcome this up to a great extent but being high temperature processes, they put many fabrication and technological limits in device fabrication. Especially keeping an eye on the future flexible devices, herein we report ultraviolet-ozone (UVO) annealing as a room-temperature, simple and cost-effective annealing method to improve the optical efficiency of ZnO and ZnMgO nanorods along with control of defect states. The ZnO and ZnMgO nanorods were grown by hydrothermal method and annealed in UVO irradiation. UVO annealing substantially improved near band emission and suppressed defect band emissions. It is found that zinc interstitial atoms migrate from the top portion of ZnO nanorods towards the bottom of nanorods after UVO annealing, resulting in reduced zinc interstitial defects in the top portion of nanorods. X-ray diffraction results showed improvement in structural properties. XPS results confirmed suppression of oxygen vacancies and zinc interstitials and improvement in lattice oxygen in the ZnO nanorods after UVO annealing. Optimum times of UVO annealing for ZnO and ZnMgO nanorods were 30 and 50 min respectively. These findings will be helpful for the further development of ZnO and ZnMgO nanorods based high performance optoelectronic devices and sensors. © 2020, Springer Science+Business Media, LLC, part of Springer Nature.Item Detection of acceptor-bound exciton peak at 300 K in boron–phosphorus co-doped ZnMgO thin films for room-temperature optoelectronics applications(Elsevier B.V., 2021) Sushama, S.; Murkute, P.; Ghadi, H.; Pandey, S.K.; Chakrabarti, S.It is well-known that the ZnMgO thin-film faces a roadblock in its potential applications for various optoelectronic devices due to the limitation imposed on achieving p-type conduction. The mono-acceptor doping of ZnMgO endures from the stern self-compensation by native donor defects and deep acceptor level formation advocating the need for alternate doping techniques like co-doping. In this paper, we report a detailed study on the improvement in structural, elemental, and optical properties of phosphorus-doped Zn0.85Mg0.15O thin films, with an aim to obtain enhancement in the signatures of acceptor-doped behavior, under the influence of boron implantation time. In addition, the paper also captures the behavior exhibited by the co-doped samples as a result of the variation in the annealing temperature. The solubility of the phosphorus atom (acceptor dopant) was observed to improve with boron (donor co-dopant) implantation as confirmed by the structural, elemental, and optical properties of co-doped ZnMgO thin films. It was also found that the acceptor level emissions got improved after boron implantation in phosphorus-doped ZnMgO thin films. Additionally, with co-doping, the sample showed the signature of acceptor-bound exciton peak till 300 K, evidencing the room-temperature operability of the films. Moreover, the fabricated film had a shallow acceptor energy level located at around 74 ± 0.45 meV above the valence band. Co-doped samples also showed stable acceptor based optical emission for more than a year. © 2020 Elsevier B.V.Item Growth of Very Large MoS2Single Crystals Using Out-Diffusion Transport and Their Use in Field Effect Transistors(Institute of Electrical and Electronics Engineers Inc., 2021) Pandey, S.K.; Izquierdo, N.; Campbell, S.Monolayer molybdenum disulfide (MoS2) is an attractive 2D material with a wide range of potential applications in the field of electronics and optoelectronics. To obtain the best performance, it is very necessary to grow large area single crystals of MoS2 (single domain) to avoid the effects of grain boundaries, but is exceptionally challenging to do this. Here, we report a novel method which we call out-diffusion vapor transport to grow large area single crystal monolayer MoS2 using an otherwise conventional chemical vapor deposition system. In this method, microchannels were created on the boat to significantly limit the region where MoOx vapor can react with S vapor to form crystals. This growth method resulted in triangular monolayer MoS2 single crystals up to ?640 ?m on a side grown on an oxidized silicon substrate, the largest crystals reported to date. Most of these crystals were multilayer at the center. This common feature has been identified in the literature as partially reduced transition metal oxide nucleates a second layer. We also achieved fully monolayer MoS2 single crystals up to ?450 ?m on a side, the largest demonstrated without the MoOx. Fabricated field effect transistors (FET) using MoS2 monolayer crystal as the active layer demonstrate a conventional n-type behavior, room-temperature mobility up to 45.5 cm2 V-1 s-1 and a maximum ON-Current (ION)/OFF-current (IOFF) ratio of 1.8 × 107. Raman and Photoluminescence results indicate that the as-grown large area monolayer crystals have high crystalline quality and uniformity with minimal defects, a finding that is consistent with the high electron mobility. This research work provides a superior technique to grow large-area high-quality single-crystal monolayer MoS2 without resorting to exotic equipment or techniques. © 2002-2012 IEEE.Item Experimental investigation and comparative analysis of electron beam evaporated ZnO/MgxZn1-xO/CdxZn1-xO thin films for photodiode applications(Academic Press, 2021) Kumar, R.R.; Shukla, R.; Pandey, S.K.; Pandey, S.K.— This work reports the growth optimization and analysis of ZnO, MgxZn1-xO, and CdxZn1-xO thin films on silicon substrate using an electron beam evaporation system. The crystal phase purity, surface morphology, optical and electrical properties of deposited ZnO, MgxZn1-xO, and CdxZn1-xO thin films were studied. X-ray diffraction (XRD) spectra revealed that the deposited films were polycrystalline in nature with preferred (002) crystal orientation. Field emission scanning electron microscope study showed a dense-packed grained structure with an exact symmetrical distribution. The root-mean-square roughness of 3.03 nm was perceived by atomic force microscopy measurement for MgxZn1-xO thin-film, indicating good morphology of the deposited film. Photoluminescence measurement demonstrated a near-band-edge emission peak around 363 nm for ZnO thin film. The energy band gap obtained for ZnO, MgxZn1-xO, and CdxZn1-xO were 3.36 eV, 3.86 eV, and 2.89 eV, respectively, as measured by Ultraviolet–Visible spectroscopy. The higher amount of photocurrent was detected in illumination condition compared to dark condition with responsivity 0.54 AW-1 for ZnO films, making it suitable for photodiodes applications. © 2020 Elsevier LtdItem Phosphorus doping of ZnO using spin-on dopant process: A better choice than costly and destructive ion-implantation technique(Elsevier B.V., 2021) Mishra, M.; Sushama, S.; Pandey, S.K.; Chakrabarti, S.Radio frequency sputtered ZnO thin films doped with phosphorus (ZnO:P) have been prepared employing spin-on dopant process. In the SOD process, the dopant film has been spin-coated on a silicon substrate and positioned close to the as-deposited undoped ZnO film at high temperature to perform the phosphorus doping. The high-resolution X-ray diffraction measurement reveals that the prepared ZnO:P films are good in crystalline quality which improves further by annealing. It is found that the full-width half-maximum corresponding to (002) peak of SOD processed thin films is much narrower than previously reported ion-implanted thin films, indicating the better crystalline quality of SOD processed phosphorus-doped ZnO thin films. The X-ray photoelectron spectroscopy measurement signifies that the P2O5 decomposes into two phosphorus atoms behaving like an acceptor dopant and five oxygen atoms which may fill in oxygen vacancies at high-temperature annealing. The photoluminescence spectra discover the acceptor bound exciton peak at 3.35 eV and free electron to acceptor level transitions at 3.31 eV. The calculated acceptor binding energy is 127 meV for the phosphorus dopant which works as a shallow acceptor level. It is found that the phosphorus-doped ZnO thin films prepared using the SOD process have much superior structural and optical properties in comparison to previously reported ion-implanted film. This study demonstrates that the SOD process is much superior than the ion-implantation process to produce high-quality ZnO:P thin films for very stable p-type conduction. © 2021 Elsevier B.V.Item Improving the Cu2ZnSn(S,Se)4-Based Photovoltaic Conversion Efficiency by Back-Contact Modification(Institute of Electrical and Electronics Engineers Inc., 2021) Sengar, B.S.; Garg, V.; Siddharth, G.; Kumar, A.; Pandey, S.K.; Dubey, M.; Atuchin, V.V.; Kumar, S.; Mukherjee, S.Back-contact modification using a 10-nm ZnS layer in CZTSSe-based solar cell can play a crucial role in improving photovoltaic conversion efficiency. An ultrathin layer of ZnS is deposited over Mo-coated soda lime glass substrate before depositing CZTSSe using sputtering. The crystal structure of deposited CZTSSe thin films over ZnS is recognized as (112)-oriented, polycrystalline in nature, and free from the presence of any secondary phases such as Cu2(S,Se) or Zn(S,Se). The bandgap of CZTSSe thin films deposited over ultrathin ZnS is observed to increase from 1.49 (deposited over Mo directly) to 1.58 eV at room temperature, as determined by spectroscopic ellipsometry. In addition, numerical simulation has been performed using SCAPS software. The impact of ZnS layer has been simulated by using the defects in the absorber and at the interface of ZnS/CZTSSe. The simulated results have been validated with experimentally fabricated CZTSSe device. Simulated device with ZnS intermediate layer is observed to give rise to a photovoltaic conversion efficiency of 15.2%. © 1963-2012 IEEE.Item Theoretical investigations of band alignments and SnSe BSF layer for low-cost, non-toxic, high-efficiency CZTSSe solar cell(Elsevier Ltd, 2021) Prabhu, S.; Pandey, S.K.; Chakrabarti, S.In this work, a numerical simulation approach is utilized using SCAPS-1D software to model, modify, optimize, and evaluate the CZTSSe solar cell structure. For the CZTSSe solar cell, one possible reason hindering the performance is improper band alignment between the absorber and the buffer layers. With conventional CdS as a buffer layer, having a fixed bandgap, tuning the band alignment is impossible. To overcome this issue, Cd-free zinc oxide-based compounds Zn(O1-xSx), Zn1-xSnxO, and Zn1-xMgxO are explored as buffer layers, and their performance is evaluated. Using their composition-dependent tunable bandgap as an advantage, suitable band alignment with the absorber layer is evaluated for equal or higher performance when compared to CdS. Further performance improvement is attempted by using SnSe as the back surface field (BSF) layer. Band alignment evaluation is also extended to the back contact (Mo)/SnSe interface, whereby an attempt is made to replace Mo with a suitable metal. The Ni is found as a good candidate to replace Mo to achieve high-efficiency solar cell. The same approach is repeated with the transparent conducting oxide layer, and aluminum doped zinc oxide (AZO) is found as a suitable material in place of ITO for optimized solar cell structure. A maximum power conversion efficiency of 17.55% is achieved with an optimized structure. It is also observed that the external quantum efficiency (EQE) of the solar cell is improved significantly in the blue photons region in comparison to the EQE of the champion solar cell. The optimized structure Ni/SnSe/CZT(S0.4Se0.6)/Zn(O0.3S0.7)/i-ZnO/AZO in this work will be very useful to fabricate low-cost and Cd-free high-efficiency kesterite solar cells. © 2021Item Enhancement in structural, elemental and optical properties of boron–phosphorus Co-doped ZnO thin films by high-temperature annealing(Elsevier B.V., 2021) Sushama, S.; Murkute, P.; Ghadi, H.; Pandey, S.K.; Chakrabarti, S.The inherent n-type nature of zinc oxide (ZnO) and its unstable p-type behavior with single dopant species have encouraged researchers to explore the effect of multiple dopants as a viable solution for long-term stability and repeatability. Herein, we report boron (B) and phosphorus (P) co-doped ZnO thin films engineered through an optimized ion implantation technique followed by annealing at 1000 °C in oxygen ambiance. We investigated their structural, chemical, and optical properties to capture the effect of both boron implantation duration and annealing temperature. Co-doping with boron was observed to boost phosphorus incorporation in the film. Compared with P-doping, P–B co-doping increased the dominance of acceptor-bound exciton peak and also, suppressed non-radiative/visible emission which is due to reduced Madelung energy. After high-temperature annealing at 1000 °C, further narrowing of optical emission peaks generated due to acceptor incorporation was observed. Also, the co-doped samples showed stability in the acceptor behavior for more than one year. © 2021 Elsevier B.V.Item Large and Uniform Single Crystals of MoS2Monolayers for ppb-Level NO2Sensing(American Chemical Society, 2022) Patel, C.; Singh, R.; Dubey, M.; Pandey, S.K.; Upadhyay, S.N.; Kumar, V.; Sriram, S.; Than Htay, M.; Pakhira, S.; Atuchin, V.V.; Mukherjee, S.Recently, unprecedented interest has been immersed toward the synthesis of two-dimensional (2D) transition metal dichalcogenides via the chemical vapor deposition (CVD) system. Synthesis of a uniform and large-sized monolayer MoS2atomic thin film via CVD is still a major bottleneck owing to strong dependence on diverse associated growth parameters. In this work, we have proposed the most viable recipe which is suitable for controlling the nucleation density of Mo and producing a 90 μm-long MoS2monolayer crystal and (695 × 394.8) μm2large MoS2monolayered film on SiO2/Si and c-plane sapphire, respectively. Moreover, MoS2monolayer sensing performance has been thoroughly investigated for NO2exposure at room temperature with a varying response of 4-57.5 for the 100-100 ppm level. Furthermore, the MoS2monolayer sensor exhibits an ultrasensitive NO2detection with limit of detection and limit of qualification values of 1.4 and 4.6 ppb, respectively. In addition, the first-principles-based density functional theory has been employed to analyze the adsorption of NO2on the surfaces of the 2D MoS2monolayer. It is observed that the electronic band gap of the MoS2monolayer after NO2adsorption is reduced by 0.7 eV due to molecular orbital hybridization. © 2022 American Chemical Society. All rights reserved.Item Innovative structural engineering of sustainable and environment-friendly Cu2ZnSnS4 solar cell for over 20% conversion efficiency(John Wiley and Sons Ltd, 2022) Prabhu, S.; Pandey, S.K.; Chakrabarti, S.Kesterite Cu2ZnSnS4(CZTS) thin-film technology has been comprehensively investigated over the last decade as a promising candidate in the field of photovoltaic technologies. However, despite numerous strategies to improve the performance, the efficiencies remain stagnant at around 11%. Poorly optimized absorber/buffer interface, non-absorption of higher wavelength photons, and non-ohmic back contact are the primary reasons for the poor performance of the CZTS solar cell. The authors of this paper propose a cadmium-free buffer layer, multiple quantum wells (MQWs) structure, and a back surface field (BSF) layer to overcome these issues, respectively. In this study, the buffer layer, zinc oxysulfide (Zn[O1−xSx]) is considered as an alternative to toxic Cadmium Sulfide (CdS) for better band alignment with the CZTS absorber layer. Cu2ZnSn(SxSe1−x)4 (CZTSSe) is used as a quantum well material in MQWs to increase photon absorption in CZTS solar cells. Tin selenide (SnSe) is used as the BSF layer to reduce the effect of non-ohmic back contact and to improve the open-circuit voltage (Voc) of MQW incorporated CZTS solar cells. Detailed analysis and optimization of the modified structure with higher performance are presented. The simulation results obtained provide imperative guidelines for the fabrication of high-efficiency CZTS solar cells using non-toxic and earth-abundant materials. © 2022 John Wiley & Sons Ltd.